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arXiv:2503.20872

Hybrid interfaces at the single quantum level in fluorescent molecules

Daniele De Bernardis, Hugo Levy-Falk, Elena Fanella, Rocco Duquennoy, Valerio Digiorgio, Giacomo Scalari, Maja Colautti, Costanza Toninelli

Published Mar 26, 2025• 0 citations
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Abstract

We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.

DOI
10.48550/arxiv.2503.20872

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We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.
We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.
Abstract We theoretically investigate a single fluorescent molecule as a hybrid quantum optical device, in which multiple external laser sources exert control of the vibronic states. In the high-saturation regime, a coherent interaction is established between the vibrational and electronic degrees of freedom, and molecules can simulate several cavity QED models, whereby a specific vibrational mode plays the role of the cavity mode. Focusing on the specific example where the system is turned into an analogue simulator of the quantum Rabi model, the steady state exhibits vibrational bi-modality resulting in a statistical mixture of highly non-classical vibronic cat states. Applying our paradigm to molecules with prominent spatial asymmetry and combining an optical excitation with a THz(IR) driving, the system can be turned into a single photon transducer. Two possible implementations are discussed based on the coupling to a subwavelength THz patch antenna or a resonant metamaterial. In a nutshell, this work assesses the role of molecules as an optomechanical quantum toolbox for creating hybrid entangled states of electrons, photons, and vibrations, hence enabling frequency conversion over very different energy scales.
We identify enhanced strong coherent Surface-Enhanced Raman Scattering (SERS) interactions facilitated by hybridized metallo-dielectric cavities with a resonant fluorescent molecule. By illuminating a detuned electronic transition near saturation via a narrowband hybrid plasmonic mode, we observe enhanced splittings in the Stokes and anti-Stokes spectra, revealing strong optomechanical coupling and nonlinear vibrational modifications at intensities far below irreversible SERS damage thresholds. We compute the second-order photon correlations that allows identifying the nonclassical character associated to these strong optomechanical interactions and SERS configurations that enables them to optically characterize the anharmonic character of the vibrational modes.
Macroscopic entangled cat states not only are significant in the demonstration of the fundamentals of quantum physics, but also have wide applications in modern quantum technologies such as continuous-variable quantum information processing and quantum metrology. Here we propose a scheme for generation of macroscopic entangled cat states in a longitudinal-coupled cavity-QED model. In particular, we introduce the scheme by using the terms of a molecular cavity-QED system, which is composed of an organic molecule (including electronic and vibrational states) coupled to a single-mode cavity field. In this system, the resonance frequencies of the molecular vibration and the cavity field are modulated simultaneously, then the molecular vibrational displacement is enhanced significantly and hence macroscopic entangled cat states between the molecular vibrational mode and the cavity mode can be created. We also study quantum coherence effects in the generated states by calculating the joint Wigner function and the degree of entanglement. The dissipation effects are included by considering the state generation in the open-system case. Our results will pave the way to the study of quantum physics and quantum chemistry in molecular cavity-QED systems. The physical mechanism behind this scheme is general and can be extended to other longitudinal-coupled cavity-QED systems.
We propose a scheme to realize frequency conversion of photons, using a hybrid system with a qubit coupled to both a resonator cavity and an optomechanical cavity. In this system, a high-energy photon can be converted into a low-energy photon plus a phonon and vice versa; the qubit works as an intermediate medium with its states unchanged. Moreover, the process can be exquisitely tuned by changing the frequency of the qubit or the resonator mode, providing additional control for the conversion. We further analyze the system dynamics and demonstrate two Rabi oscillation behaviors with dissipations. With the state-of-the-art techniques in cavity quantum electrodynamics and optomechanical systems, our proposal would be implemented and an efficient and controllable quantum light source can be achieved.
We show that an atom can be coupled to a mechanical oscillator via quantum vacuum fluctuations of a cavity field enabling energy transfer processes between them. In a hybrid quantum system consisting of a cavity resonator with a movable mirror and an atom, these processes are dominated by two pair-creation mechanisms: the counterrotating (atom-cavity system) and dynamical Casimir interaction terms (optomechanical system). Because of these two pair-creation mechanisms, the resonant atom-mirror coupling is the result of high-order virtual processes with different transition paths well described in our theoretical framework. We perform a unitary transformation to the atom-mirror system Hamiltonian, exhibiting two kinds of multiple-order transitions of the pair creation. By tuning the frequency of the atom, we show that photon frequency conversion can be realized within a cavity of multiple modes. Furthermore, when involving two atoms coupled to the same mechanical mode, a single vibrating excitation of the mechanical oscillator can be simultaneously absorbed by the two atoms. Considering recent advances in strong and ultrastrong coupling for cavity optomechanics and other systems, we believe our proposals can be implemented using available technology.